Direct observation of the energy gain underpinning ferromagnetic superexchange in the electronic structure of CrGeTe${}_3$

Abstract

We investigate the temperature-dependent electronic structure of the van der Waals ferromagnet, CrGeTe${}_3$. Using angle-resolved photoemission spectroscopy, we identify atomic- and orbital-specific band shifts upon cooling through $T_{\mathrm{C}}$. From these, together with x-ray absorption spectroscopy and x-ray magnetic circular dichroism measurements, we identify the states created by a covalent bond between the Te $5p$ and the Cr $e_g$ orbitals as the primary driver of the ferromagnetic ordering in this system, while it is the Cr $t_{2g}$ states that carry the majority of the spin moment. The $t_{2g}$ states furthermore exhibit a marked bandwidth increase and a remarkable lifetime enhancement upon entering the ordered phase, pointing to a delicate interplay between localized and itinerant states in this family of layered ferromagnets.

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• Giant exchange splitting in the electronic structure of A-type 2D antiferromagnet CrSBr
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• The planar triangular $S=3/2$ magnet AgCrSe${}_2$: magnetic frustration, short range correlations, and field tuned anisotropic cycloidal magnetic order
• Spectral Evidence for Local-Moment Ferromagnetism in van der Waals Metals Fe${}_3$GaTe${}_2$ and Fe${}_3$GeTe${}_2$
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• Electrical tuning of the magnetic properties of 2D magnets: the case of ${\mathrm{Cr}}_2{\mathrm{Ge}}_2{\mathrm{Te}}_6$
• Flux-pinning mediated superconducting diode effect in the NbSe${}_2$/CrGeTe${}_3$ heterostructure
• Two-Step Electronic Response to Magnetic Ordering in a van der Waals Ferromagnet
• Orbital magnetization in two-dimensional materials from high-throughput computational screening
• X-ray spectra in magnetic van der Waals materials Fe${}_3$GeTe${}_2$, CrI${}_3$, and CrGeTe${}_3$: a first-principles study
• Charge doping into spin minority states mediates doubling of $T_{\mathrm{C}}$ in ferromagnetic CrGeTe${}_3$
• Near room-temperature ferromagnetism from double-exchange in the van der Waals material CrGeTe${}_3$: evidence from optical conductivity under pressure
• Electronic structure of monolayer-CrTe${}_2$: an antiferromagnetic 2D van der Waals material
• Magnetodielectric Properties in Two Dimensional Magnetic Insulators
• Phonon frequency comb close to an isolated Einstein mode in InSiTe3
• Orbital mixing and strong Hund's coupling stabilize spin order in van der Waals ferromagnet CrI3